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High syngas selectivity and near pure hydrogen production in perovskite oxygen carriers for chemical looping steam methane reforming

文献类型：期刊论文

作者Zhao, Kun1,2,5; Zhang, Rongjiang3; Gao, Yunfei4; Lin, Yan1,2,5; Liu, Anqi1,2,5; Wang, Xiaobo1,2,5; Zheng, Anqing1,2,5; Huang, Zhen1,2,5; Zhao, Zengli1,2,5
刊名FUEL PROCESSING TECHNOLOGY
出版日期2022-11-01
卷号236页码:9
ISSN号0378-3820
关键词Chemical looping Methane reforming Hydrogen Oxygen vacancy
DOI10.1016/j.fuproc.2022.107398
通讯作者Zheng, Anqing(zhengaq@ms.giec.ac.cn) ; Huang, Zhen(huangzhen@ms.giec.ac.cn)
英文摘要Chemical looping steam methane reforming (CL-SMR) provides an attractive route for hydrogen and syngas co-production through two successive steps of methane oxidation and steam splitting. However, there is also carbon formation through CH4 cracking which hampers the production of syngas (H-2 and CO) and the following pro-duction of pure H-2. This work prepared the perovskites La(0.95)Ce(0.05)NixFe(1-x)O(3) (x = 0, 0.2, 0.5, 0.8, 1.0) as oxygen carriers for CL-SMR. The methane activation and steam splitting were investigated based on reactivity tests on a fixed-bed reactor and various characterizations. Results showed that La0.95Ce0.05Ni0.2Fe0.8O3 and La0.95Ce0.05-Ni0.5Fe0.5O3 reached a high syngas selectivity (94.8%, 89.0%) accompanied with good methane conversion (93.1% and 95.7%) for methane partial oxidation, and near 100% hydrogen concentrations (higher than 99.6% and 99.5%) for steam splitting, indicating that additional separation step for pure hydrogen acquisition can be omitted. The H-2/CO molar ratio was maintained at the optimal value of 2.0 throughout the methane partial oxidation process. Characterizations and density functional theory calculations demonstrated that methane partial oxidation was promoted via an oxygen vacancy-mediated Mars-van-Krevelen type mechanism and the partial oxidation ability of the oxygen carrier is restricted by its content of oxygen vacancy and lattice oxygen migration rate. The proper amount of Ni doping forming the Ni-Fe synergetic effects also contributed highly to methane partial oxidation. Afterward, the deeply reduced metals combined with the oxygen vacancies provided active sites for steam splitting, hence generating pure H-2.
WOS关键词PERFORMANCE ; OXIDES ; CATALYST ; CO2 ; CE
资助项目National Natural Science Foundation of China[51876205] ; National Natural Science Foundation of China[51776209] ; National Natural Science Foundation of China[22179027] ; Youth Innovation Promotion Association, CAS[2019341] ; Science and Technology Program of Guangzhou[201904010128]
WOS研究方向Chemistry ; Energy & Fuels ; Engineering
语种英语
出版者ELSEVIER
WOS记录号WOS:000835233800002
资助机构National Natural Science Foundation of China ; Youth Innovation Promotion Association, CAS ; Science and Technology Program of Guangzhou
源URL[http://ir.giec.ac.cn/handle/344007/37075]  
专题中国科学院广州能源研究所
通讯作者Zheng, Anqing; Huang, Zhen
作者单位1.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou 510640, Peoples R China
2.CAS Key Lab Renewable Energy, Guangzhou 510640, Peoples R China
3.Xi An Jiao Tong Univ, Sch Chem Engn & Technol, Shanxi Key Lab Energy Chem Proc Intensifcat, Xian 710049, Shaanxi, Peoples R China
4.East China Univ Sci & Technol, Shanghai Engn Res Ctr Coal Gasificat, Key Lab Coal Gasificat & Energy Chem Engn, Minist Educ, Shanghai 200237, Peoples R China
5.Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou 510640, Peoples R China
推荐引用方式
GB/T 7714		 Zhao, Kun,Zhang, Rongjiang,Gao, Yunfei,et al. High syngas selectivity and near pure hydrogen production in perovskite oxygen carriers for chemical looping steam methane reforming[J]. FUEL PROCESSING TECHNOLOGY,2022,236:9.
APA Zhao, Kun.,Zhang, Rongjiang.,Gao, Yunfei.,Lin, Yan.,Liu, Anqi.,...&Zhao, Zengli.(2022).High syngas selectivity and near pure hydrogen production in perovskite oxygen carriers for chemical looping steam methane reforming.FUEL PROCESSING TECHNOLOGY,236,9.
MLA Zhao, Kun,et al."High syngas selectivity and near pure hydrogen production in perovskite oxygen carriers for chemical looping steam methane reforming".FUEL PROCESSING TECHNOLOGY 236(2022):9.

入库方式： OAI收割

来源：广州能源研究所

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